Dry reforming of methane over gallium-based supported catalytically active liquid metal solutions

Wolf M, de Oliveira A, Taccardi N, Maisel S, Heller M, Khan Antara S, Soegaard A, Felfer P, Görling A, Haumann M, Wasserscheid P (2023)

Publication Type: Journal article

Publication year: 2023

Journal

Communications Chemistry Nature Research

Book Volume: 6

Article Number: 224

Journal Issue: 1

DOI: 10.1038/s42004-023-01018-w

Abstract

Gallium-rich supported catalytically active liquid metal solutions (SCALMS) were recently introduced as a new way towards heterogeneous single atom catalysis. SCALMS were demonstrated to exhibit a certain resistance against coking during the dehydrogenation of alkanes using Ga-rich alloys of noble metals. Here, the conceptual catalytic application of SCALMS in dry reforming of methane (DRM) is tested with non-noble metal (Co, Cu, Fe, Ni) atoms in the gallium-rich liquid alloy. This study introduces SCALMS to high-temperature applications and an oxidative reaction environment. Most catalysts were shown to undergo severe oxidation during DRM, while Ga-Ni SCALMS retained a certain level of activity. This observation is explained by a kinetically controlled redox process, namely oxidation to gallium oxide species and re-reduction via H2 activation over Ni. Consequentially, this redox process can be shifted to the metallic side when using increasing concentrations of Ni in Ga, which strongly suppresses coke formation. Density-functional theory (DFT) based ab initio molecular dynamics (AIMD) simulations were performed to confirm the increased availability of Ni at the liquid alloy-gas interface. However, leaching of gallium via the formation of volatile oxidic species during the hypothesised redox cycles was identified indicating a critical instability of Ga-Ni SCALMS for prolonged test durations.

Authors with CRIS profile

Moritz Wolf Lehrstuhl für Chemische Reaktionstechnik Ana de Oliveira Lehrstuhl für Chemische Reaktionstechnik Nicola Taccardi Lehrstuhl für Chemische Reaktionstechnik Sven Maisel Lehrstuhl für Theoretische Chemie Martina Heller Lehrstuhl für Werkstoffwissenschaften (Allgemeine Werkstoffeigenschaften) Sharmin Khan Antara Lehrstuhl für Chemische Reaktionstechnik Alexander Soegaard Lehrstuhl für Chemische Reaktionstechnik Peter Felfer Professur für Atom Probe Tomography Andreas Görling Lehrstuhl für Theoretische Chemie Marco Haumann Lehrstuhl für Chemische Reaktionstechnik Peter Wasserscheid Lehrstuhl für Chemische Reaktionstechnik

How to cite

APA:

Wolf, M., de Oliveira, A., Taccardi, N., Maisel, S., Heller, M., Khan Antara, S.,... Wasserscheid, P. (2023). Dry reforming of methane over gallium-based supported catalytically active liquid metal solutions. Communications Chemistry, 6(1). https://doi.org/10.1038/s42004-023-01018-w

MLA:

Wolf, Moritz, et al. "Dry reforming of methane over gallium-based supported catalytically active liquid metal solutions." Communications Chemistry 6.1 (2023).

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